Abstract

We report a study of two nonlinear optical processes at the nanoscale level, using a near-field probe: (i) two-photon-pumped upconversion from ZnS:Mn nanoparticles encapsulated with 2ϵ24ethylsulfonylphenyl1ethenylmethylanilino1ethanethiol and (ii) second-harmonic generation (SHG) from N-(4-nitrophenyl)-L-prolinol crystallites. The use of highly efficient nonlinear organic chromophores together with special processing on the nanometer scale made it possible to observe and characterize what are believed to be the smallest topographically distinguishable objects reported so far, using nonlinear optical techniques. Issues pertaining to the study of two-photon-excited emission and SHG by use of a near-field probe are discussed.

© 1999 Optical Society of America

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  1. U. Schwarz, M. L. Berthié, D. Courjon, and H. Bielefeldt, Opt. Commun. 134, 301 (1997).
    [CrossRef]
  2. A. Klini, T. David, E. Bourillot, S. Emonin, P. Papadopoulos, J. P. Goudonnet, and G. Kotrotsios, J. Lightwave Technol. 16, 1220 (1998).
    [CrossRef]
  3. D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
    [CrossRef]
  4. M. R. Shortreed, S. Dourado, and R. Kopelman, Sensors Actuators B 38, 8 (1997).
    [CrossRef]
  5. M. Jacoby, Chem. Eng. News 76(47), 38 (1998).
    [CrossRef]
  6. A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
    [CrossRef]
  7. D. A. Vanden Bout, J. Kerimo, D. A. Higgins, and P. F. Barbara, Acc. Chem. Res. 30, 204 (1997).
    [CrossRef]
  8. B. Hecht, D. W. Pohl, H. Heinzelmann, and L. Novotny, Ultramicroscopy 61, 99 (1995).
    [CrossRef]
  9. M. K. Lewis, P. Wolanin, A. Gafni, and D. G. Steel, Opt. Lett. 23, 1111 (1998).
    [CrossRef]
  10. T. K. De and A. Maitra, Adv. Colloid Interface Sci. 59, 95 (1995).
    [CrossRef]
  11. L. C. Klein, ed., Sol-Gel Technology for Thin Films, Fibers, Preforms, Electronics and Specialty Shapes (Noyes, Park Ridge, New Jersey, 1988).
  12. L. Novotny, “Light propagation and light confinement in near-field optics,” Ph.D. dissertation (Eidgenössische Technische Hochschule Zürich, Zurich, 1996).
  13. J. ?wia?tkiewicz, P. N. Prasad, and B. A. Reinhardt, Opt. Commun. 157, 135 (1998).
    [CrossRef]
  14. J. Zyss, J. F. Nicoud, and M. Coquillay, J. Chem. Phys. 81, 4160 (1984).
    [CrossRef]
  15. P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
    [CrossRef]
  16. M. Adameck, R. Blum, and M. Eich, Appl. Phys. Lett. 73, 2884 (1998).
    [CrossRef]
  17. I. I. Smolyaninov, A. V. Zayats, and C. C. Davis, Phys. Rev. B 56, 9290 (1997).
    [CrossRef]

1998 (5)

A. Klini, T. David, E. Bourillot, S. Emonin, P. Papadopoulos, J. P. Goudonnet, and G. Kotrotsios, J. Lightwave Technol. 16, 1220 (1998).
[CrossRef]

M. Jacoby, Chem. Eng. News 76(47), 38 (1998).
[CrossRef]

M. K. Lewis, P. Wolanin, A. Gafni, and D. G. Steel, Opt. Lett. 23, 1111 (1998).
[CrossRef]

J. ?wia?tkiewicz, P. N. Prasad, and B. A. Reinhardt, Opt. Commun. 157, 135 (1998).
[CrossRef]

M. Adameck, R. Blum, and M. Eich, Appl. Phys. Lett. 73, 2884 (1998).
[CrossRef]

1997 (5)

I. I. Smolyaninov, A. V. Zayats, and C. C. Davis, Phys. Rev. B 56, 9290 (1997).
[CrossRef]

U. Schwarz, M. L. Berthié, D. Courjon, and H. Bielefeldt, Opt. Commun. 134, 301 (1997).
[CrossRef]

D. A. Vanden Bout, J. Kerimo, D. A. Higgins, and P. F. Barbara, Acc. Chem. Res. 30, 204 (1997).
[CrossRef]

D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
[CrossRef]

M. R. Shortreed, S. Dourado, and R. Kopelman, Sensors Actuators B 38, 8 (1997).
[CrossRef]

1996 (1)

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

1995 (2)

B. Hecht, D. W. Pohl, H. Heinzelmann, and L. Novotny, Ultramicroscopy 61, 99 (1995).
[CrossRef]

T. K. De and A. Maitra, Adv. Colloid Interface Sci. 59, 95 (1995).
[CrossRef]

1992 (1)

P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
[CrossRef]

1984 (1)

J. Zyss, J. F. Nicoud, and M. Coquillay, J. Chem. Phys. 81, 4160 (1984).
[CrossRef]

Adameck, M.

M. Adameck, R. Blum, and M. Eich, Appl. Phys. Lett. 73, 2884 (1998).
[CrossRef]

Andreazza, P.

P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
[CrossRef]

Barbara, P. F.

D. A. Vanden Bout, J. Kerimo, D. A. Higgins, and P. F. Barbara, Acc. Chem. Res. 30, 204 (1997).
[CrossRef]

Benami, N. K.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Benami, U.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Berthié, M. L.

U. Schwarz, M. L. Berthié, D. Courjon, and H. Bielefeldt, Opt. Commun. 134, 301 (1997).
[CrossRef]

Bielefeldt, H.

U. Schwarz, M. L. Berthié, D. Courjon, and H. Bielefeldt, Opt. Commun. 134, 301 (1997).
[CrossRef]

Blum, R.

M. Adameck, R. Blum, and M. Eich, Appl. Phys. Lett. 73, 2884 (1998).
[CrossRef]

Bourillot, E.

Coquillay, M.

J. Zyss, J. F. Nicoud, and M. Coquillay, J. Chem. Phys. 81, 4160 (1984).
[CrossRef]

Courjon, D.

U. Schwarz, M. L. Berthié, D. Courjon, and H. Bielefeldt, Opt. Commun. 134, 301 (1997).
[CrossRef]

David, T.

Davis, C. C.

I. I. Smolyaninov, A. V. Zayats, and C. C. Davis, Phys. Rev. B 56, 9290 (1997).
[CrossRef]

De, T. K.

T. K. De and A. Maitra, Adv. Colloid Interface Sci. 59, 95 (1995).
[CrossRef]

Deckert, V.

D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
[CrossRef]

Dourado, S.

M. R. Shortreed, S. Dourado, and R. Kopelman, Sensors Actuators B 38, 8 (1997).
[CrossRef]

Druckmann, S.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Dutoit, B.

D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
[CrossRef]

Eich, M.

M. Adameck, R. Blum, and M. Eich, Appl. Phys. Lett. 73, 2884 (1998).
[CrossRef]

Emonin, S.

Fish, G.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Gafni, A.

Goudonnet, J. P.

Hecht, B.

B. Hecht, D. W. Pohl, H. Heinzelmann, and L. Novotny, Ultramicroscopy 61, 99 (1995).
[CrossRef]

Heinzelmann, H.

B. Hecht, D. W. Pohl, H. Heinzelmann, and L. Novotny, Ultramicroscopy 61, 99 (1995).
[CrossRef]

Higgins, D. A.

D. A. Vanden Bout, J. Kerimo, D. A. Higgins, and P. F. Barbara, Acc. Chem. Res. 30, 204 (1997).
[CrossRef]

Jacoby, M.

M. Jacoby, Chem. Eng. News 76(47), 38 (1998).
[CrossRef]

Josse, D.

P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
[CrossRef]

Kerimo, J.

D. A. Vanden Bout, J. Kerimo, D. A. Higgins, and P. F. Barbara, Acc. Chem. Res. 30, 204 (1997).
[CrossRef]

Khachatryan, E.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Klini, A.

Kopelman, R.

M. R. Shortreed, S. Dourado, and R. Kopelman, Sensors Actuators B 38, 8 (1997).
[CrossRef]

Kotrotsios, G.

Lefaucheux, F.

P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
[CrossRef]

Lewis, A.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Lewis, M. K.

Lieberman, K.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Maitra, A.

T. K. De and A. Maitra, Adv. Colloid Interface Sci. 59, 95 (1995).
[CrossRef]

Nicoud, J. F.

J. Zyss, J. F. Nicoud, and M. Coquillay, J. Chem. Phys. 81, 4160 (1984).
[CrossRef]

Novotny, L.

B. Hecht, D. W. Pohl, H. Heinzelmann, and L. Novotny, Ultramicroscopy 61, 99 (1995).
[CrossRef]

L. Novotny, “Light propagation and light confinement in near-field optics,” Ph.D. dissertation (Eidgenössische Technische Hochschule Zürich, Zurich, 1996).

Ottolenghi, M.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Papadopoulos, P.

Pohl, D. W.

B. Hecht, D. W. Pohl, H. Heinzelmann, and L. Novotny, Ultramicroscopy 61, 99 (1995).
[CrossRef]

Prasad, P. N.

J. ?wia?tkiewicz, P. N. Prasad, and B. A. Reinhardt, Opt. Commun. 157, 135 (1998).
[CrossRef]

Reinhardt, B. A.

J. ?wia?tkiewicz, P. N. Prasad, and B. A. Reinhardt, Opt. Commun. 157, 135 (1998).
[CrossRef]

Robert, M. C.

P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
[CrossRef]

Roth, T.

D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
[CrossRef]

Schwarz, U.

U. Schwarz, M. L. Berthié, D. Courjon, and H. Bielefeldt, Opt. Commun. 134, 301 (1997).
[CrossRef]

Shalom, S.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Shortreed, M. R.

M. R. Shortreed, S. Dourado, and R. Kopelman, Sensors Actuators B 38, 8 (1997).
[CrossRef]

Smolyaninov, I. I.

I. I. Smolyaninov, A. V. Zayats, and C. C. Davis, Phys. Rev. B 56, 9290 (1997).
[CrossRef]

Steel, D. G.

Strinkovski, A.

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

Swia¸tkiewicz, J.

J. ?wia?tkiewicz, P. N. Prasad, and B. A. Reinhardt, Opt. Commun. 157, 135 (1998).
[CrossRef]

Vanden Bout, D. A.

D. A. Vanden Bout, J. Kerimo, D. A. Higgins, and P. F. Barbara, Acc. Chem. Res. 30, 204 (1997).
[CrossRef]

Wolanin, P.

Zayats, A. V.

I. I. Smolyaninov, A. V. Zayats, and C. C. Davis, Phys. Rev. B 56, 9290 (1997).
[CrossRef]

Zeisel, D.

D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
[CrossRef]

Zenobi, R.

D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
[CrossRef]

Zyss, J.

P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
[CrossRef]

J. Zyss, J. F. Nicoud, and M. Coquillay, J. Chem. Phys. 81, 4160 (1984).
[CrossRef]

Acc. Chem. Res. (1)

D. A. Vanden Bout, J. Kerimo, D. A. Higgins, and P. F. Barbara, Acc. Chem. Res. 30, 204 (1997).
[CrossRef]

Adv. Colloid Interface Sci. (1)

T. K. De and A. Maitra, Adv. Colloid Interface Sci. 59, 95 (1995).
[CrossRef]

Anal. Chem. (1)

D. Zeisel, B. Dutoit, V. Deckert, T. Roth, and R. Zenobi, Anal. Chem. 69, 749 (1997).
[CrossRef]

Appl. Phys. Lett. (1)

M. Adameck, R. Blum, and M. Eich, Appl. Phys. Lett. 73, 2884 (1998).
[CrossRef]

Chem. Eng. News (1)

M. Jacoby, Chem. Eng. News 76(47), 38 (1998).
[CrossRef]

Isr. J. Chem. (1)

A. Lewis, K. Lieberman, N. K. Benami, G. Fish, E. Khachatryan, A. Strinkovski, S. Shalom, S. Druckmann, M. Ottolenghi, and U. Benami, Isr. J. Chem. 36, 89 (1996).
[CrossRef]

J. Chem. Phys. (1)

J. Zyss, J. F. Nicoud, and M. Coquillay, J. Chem. Phys. 81, 4160 (1984).
[CrossRef]

J. Lightwave Technol. (1)

Opt. Commun. (2)

U. Schwarz, M. L. Berthié, D. Courjon, and H. Bielefeldt, Opt. Commun. 134, 301 (1997).
[CrossRef]

J. ?wia?tkiewicz, P. N. Prasad, and B. A. Reinhardt, Opt. Commun. 157, 135 (1998).
[CrossRef]

Opt. Lett. (1)

Phys. Rev. B (2)

P. Andreazza, D. Josse, F. Lefaucheux, M. C. Robert, and J. Zyss, Phys. Rev. B 45, 7640 (1992).
[CrossRef]

I. I. Smolyaninov, A. V. Zayats, and C. C. Davis, Phys. Rev. B 56, 9290 (1997).
[CrossRef]

Sensors Actuators B (1)

M. R. Shortreed, S. Dourado, and R. Kopelman, Sensors Actuators B 38, 8 (1997).
[CrossRef]

Ultramicroscopy (1)

B. Hecht, D. W. Pohl, H. Heinzelmann, and L. Novotny, Ultramicroscopy 61, 99 (1995).
[CrossRef]

Other (2)

L. C. Klein, ed., Sol-Gel Technology for Thin Films, Fibers, Preforms, Electronics and Specialty Shapes (Noyes, Park Ridge, New Jersey, 1988).

L. Novotny, “Light propagation and light confinement in near-field optics,” Ph.D. dissertation (Eidgenössische Technische Hochschule Zürich, Zurich, 1996).

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Figures (3)

Fig. 1
Fig. 1

Topography (top) and two-photon NSOM image (bottom) of ZnS:Mn particles coated with APSS-SH. A well-defined spherical particle of 240-nm diameter and its fluorescent image are indicated by arrows.

Fig. 2
Fig. 2

Spectrum revealing the SH and the fundamental band (the latter is suppressed by 106 with filters) (solid curve). This spectrum was gathered with NSOM from a micrometer-sized object. Broadband emission generated in the fiber (with the tip) is shown by the dotted curve. A BG18 filter was used to suppress wavelengths above 550 nm.

Fig. 3
Fig. 3

Topography (top) and SH NSOM image (bottom) of a sample containing NPP. A gap of 140-nm in which the NPP nanocrystals are confined (dark spot) and a corresponding emitting (bright) spot are indicated by arrows.

Equations (1)

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Pd=Pin×10-492/d,

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